Predicting intersystem crossing efficiencies of organic molecules for efficient thermally activated delayed fluorescence

Shen, Xu; Yang, Qingqing; Wan, Yifang; Chen, Runfeng; Wang, Shuang; Si, Yubing; Yang, Baocheng; Liu, Dan; Zheng, Chao; Huang, Wei

doi:10.1039/c9tc03152a

Cited by 64 publications

(73 citation statements)

References 44 publications

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“…13 An even larger DE ST value of 0.31 eV is obtained if the T 0-0 1 transition energy is taken to coincide with the first phosphorescence band maximum (77 K), while S 0-0 1 is derived from the crossing point of the absorption and fluorescence bands at 300 K. 7,42 Other TDDFT and TDA reports best agreeing with this (latter) value were DE ST values of e.g. 0.49, 0.34 and 0.46 eV, which can be obtained when using TD-oB97X/6-31G*, 30 TD-B3LYP and TD-PBE0 34 with the same basis set.…”

Section: Minima Of the Low-lying Excited Statesmentioning

confidence: 58%

“…Here it is interesting to note that functionals like CAM-B3LYP and oB97X-D yield excitation energies above 3.6 eV for this state. 34,42 At 0.17 eV above, the S 2 state is found arising from a HÀ2 -L transition. Like S 1 , the S 2 excitation has predominantly CT character, mixed with LE on the PN unit.…”

Section: Geometries and Electronic Structure At The S 0 Statementioning

confidence: 96%

“…Such studies focus on substitution effects on the electronic and excited state properties of several CDCBs performed mainly on ground state geometries. Other computational works calculate first-order SOC values in order to obtain (R)ISC rate constants via semiclassical Marcus theory using the adiabatic T 1 state 34,35 or involving the singlettriplet crossing seam 36 .…”

Section: 23 3668mentioning

confidence: 99%

“…Other theoretical reports have also assigned the T 1 state of 2CzPN with a strongly mixed CT-LE character, e.g. by using optimally tuned long-range corrected functionals and PCM 54 and uncorrected TDA-PBE0 28 and TD-B3LYP 34 functionals. In addition, Huang et al 42 have shown how the LE contribution of this state increases with the increase of the HF exchange in conventional functionals.…”

Section: Geometries and Electronic Structure At The S 0 Statementioning

confidence: 99%

“…In contrast, TD-B3LYP calculations predict this state to be located adiabatically below the S 1 state (by 0.17 eV) being the only study reporting about the participation of this state in the (R)ISC decay processes on 2CzPN. 34 Preliminary DFT/MRCI calculations locate two adiabatic triplet states (T 1 and T 2 ) below the S 1 state in the 4CzIPN TADF emitter, 12 with the T 2 state being halfway from the T 1 and S 1 states. This strongly suggests marked differences between the TADF mechanisms of both emitters: for 4CzIPN, the presence of the intermediate T 2 state helps to accelerate the (R)ISC processes, while for 2CzPN, pathways involving the adiabatic T 2 state are thermally activated.…”

Section: Minima Of the Low-lying Excited Statesmentioning

confidence: 99%

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Intersystem crossing processes in the 2CzPN emitter: a DFT/MRCI study including vibrational spin–orbit interactions

Rodriguez-Serrano

Dinkelbach

Marian

2021

Phys. Chem. Chem. Phys.

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Section: Minima Of the Low-lying Excited Statesmentioning

confidence: 58%

Section: Geometries and Electronic Structure At The S 0 Statementioning

confidence: 96%

Section: 23 3668mentioning

confidence: 99%

Section: Geometries and Electronic Structure At The S 0 Statementioning

confidence: 99%

Section: Minima Of the Low-lying Excited Statesmentioning

confidence: 99%

See 3 more Smart Citations

Intersystem crossing processes in the 2CzPN emitter: a DFT/MRCI study including vibrational spin–orbit interactions

Rodriguez-Serrano

Dinkelbach

Marian

2021

Phys. Chem. Chem. Phys.

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Modulating Non‐Radiative Deactivation via Acceptor Reconstruction to Expand High‐Efficient Red Thermally Activated Delayed Fluorescent Emitters

et al. 2022

Advanced Optical Materials

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The development of high‐efficient red thermally activated delayed fluorescent (TADF) materials is crucial to expanding their applications. Here, the acceptor reconstruction strategies of acceptor bonding and acceptor fusing in donor–acceptor‐type materials to modulate their nonradiative deactivation process and emission color for expanding high‐efficient red TADF emitters are presented. They are applied to design novel red TADF emitters TXO‐b‐TPA and TXO‐f‐TPA based on non‐red thioxanthone oxide (TXO) acceptor. Compared to TXO‐based emitter TXO‐TPA, these acceptor reconstruction strategies enable red‐shifted (48–88 nm) and efficient red TADF emission (600–640 nm). Their radiative and nonradiative transition processes can be modulated by the different molecular orbital and excited state distributions based on their acceptor structural differences, which results in a dramatic enhancement of their organic light‐emitting diode (OLED) device efficiencies from 1.21/3.63% (TXO‐f‐TPA) to 20.9% (TXO‐b‐TPA). These results confirm that the acceptor reconstruction strategies provide a viable solution for overcoming the limitations of previous red TADF emitters. Moreover, the retrieval of reported TADF materials can further demonstrate that these acceptor reconstruction strategies can be transferrable to more non‐red TADF materials to expand high‐efficient red‐shift and/or red TADF materials.

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Improving the TADF in Corannulene‐Based Emitters via Tuning the Strength of Donor and Acceptor Groups

Jacob

Varathan

et al. 2023

Advcd Theory and Sims

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In this investigation, a systematic study on the design and development of corannulene‐based thermally activated delayed fluorescence (TADF) emitters using density functional theory methods is carried out. Benzene, benzopyrazine, difluoro‐benzopyrazine, benzene‐1,2‐dithiol, and tetrasulfone are introduced on corannulene bowl as electron‐withdrawing groups to alter the electron‐accepting property of corannulene. Three different donors, viz., carbazole, phenoxazine, and 5,10‐dihydrophenazine are substituted on the rim position of corannulene to alter the absorption properties. The relationship between chemical structure and TADF property is established by evaluating the dihedral angle between donor and acceptor units, spin–orbit coupling (SOC) values, the energy difference between singlet‐triplet excited states (ΔEST), and rates of reverse intersystem crossing (kRISC). The newly designed TADF emitters show absorption in the blue to near‐IR regions depending on the strength of the donor and acceptor moieties. Careful analysis of these properties delineates the relationship between SOC values and the nature of the excited states, which is crucial for achieving high kRISC.

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Predicting intersystem crossing efficiencies of organic molecules for efficient thermally activated delayed fluorescence

Abstract: Among five methods in predicting intersystem crossing of TADF molecules, NTO similarity and n-orbital analyses based on the T1 structure were found to be efficient with low computational costs and high accuracy.

Cited by 64 publications

References 44 publications

Intersystem crossing processes in the 2CzPN emitter: a DFT/MRCI study including vibrational spin–orbit interactions

Intersystem crossing processes in the 2CzPN emitter: a DFT/MRCI study including vibrational spin–orbit interactions

Modulating Non‐Radiative Deactivation via Acceptor Reconstruction to Expand High‐Efficient Red Thermally Activated Delayed Fluorescent Emitters

Improving the TADF in Corannulene‐Based Emitters via Tuning the Strength of Donor and Acceptor Groups

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